过渡金属负载Silicalite-1分子筛的制备及其催化糠醛加氢性能研究

doi:10.19964/j.issn.1006-4990.2023-0423

Abstract

Abstract:

Furfural is an important biomass-derived platform molecule，and developing robust catalysts with high activity and stability for furfural hydrogenation is a research hotspot.However，noble metal catalysts suffer from high costs，which cannot satisfy the demand towards large-scale industrial production.Herein，the transition metal-supported Silicalite-1 zeolite catalysts were successfully synthesized by a one-step hydrothermal method，and the influence of the introduction of four different types of transition metal elements on the structure of the Silicalite-1 zeolite was studied.Comprehensive characterization results showed that the crystallinity of the zeolite was not affected by low metal loading，and the metal species were uniformly dispersed on the surface of zeolite.In the hydrogenation of furfural，Ni-based catalyst S-Ni2 showed excellent catalytic activity toward furfural transformation with 96% furfural conversion and 71% furan selectivity.Cu-based catalyst S-Cu1 showed extraordinary selectivity toward furfuryl alcohol（100%），which was much higher than that over Cu-based catalyst prepared by impregnation method（76%）.Therefore，compared with the impregnation method，one-step hydrothermal method could be used to obtain a catalyst with high selectivity，and the method wass also simple and easy to operate.This work would open up a new direction for developing highly efficient，stable，and low-cost hydrogenation catalysts，and promote the valorization of biomass.

Key words: metal-supported zeolite, Silicalite-1 zeolite, furfural hydrogenation, one-step hydrothermal method

CLC Number:

O643.36

DI Lu, WANG Weiguo, CHEN Juexian, WU Chuanshu. Study on preparation of transition metal-supported Silicalite-1 zeolite catalyst and its catalytic performance for furfural hydrogenation[J]. Inorganic Chemicals Industry, 2024, 56(4): 125-132.

Figures/Tables 10

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M	样品编号	原料物质的量配比	过渡金属（M）占 SiO₂的质量分数/%
M	样品编号	n（SiO₂）∶n（TPAOH）∶n（H₂O）∶n（MO _x ）∶n（柠檬酸）	过渡金属（M）占 SiO₂的质量分数/%
Ni	S-Ni1	1∶0.125∶30∶0.01∶0.01	1.0
	S-Ni2	1∶0.125∶30∶0.02∶0.02	2.0
	S-Ni3	1∶0.125∶30∶0.05∶0.05	4.9
	S-Ni4	1∶0.125∶30∶0.1∶0.1	9.8
Co	S-Co1	1∶0.125∶30∶0.01∶0.01	1.0
	S-Co2	1∶0.125∶30∶0.02∶0.02	2.0
	S-Co3	1∶0.125∶30∶0.05∶0.05	4.9
	S-Co4	1∶0.125∶30∶0.1∶0.1	9.8
Cu	S-Cu1	1∶0.125∶30∶0.01∶0.01	1.1
	S-Cu2	1∶0.125∶30∶0.02∶0.02	2.1
	S-Cu3	1∶0.125∶30∶0.05∶0.05	5.3
	S-Cu4	1∶0.125∶30∶0.09∶0.1	9.6
Fe	S-Fe1	1∶0.125∶30∶0.01∶0.01	0.9
	S-Fe2	1∶0.125∶30∶0.02∶0.02	1.9
	S-Fe3	1∶0.125∶30∶0.05∶0.05	4.7
	S-Fe4	1∶0.125∶30∶0.11∶0.11	10.3

样品	金属负载量^a/%	S_total^b/ （m²·g^-1）	S_micro^c/ （m²·g^-1）	S_ext^c/ （m²·g^-1）	V_micro^c/ （cm³·g^-1）
S-Ni1	1.0	389	367	22	0.173
S-Ni2	1.7	368	323	45	0.157
S-Co1	1.0	390	370	19	0.174
S-Co2	2.1	265	237	28	0.113
S-Fe1	1.1	409	383	27	0.166
S-Cu1	1.4	301	283	18	0.137

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Study on preparation of transition metal-supported Silicalite-1 zeolite catalyst and its catalytic performance for furfural hydrogenation

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